Lead zirconate titanate, Pb(Zr0.53Ti0.47)O3 (PZT), thin films were prepared by a hybrid metalorganic decomposition (MOD) solution deposition route; the effects of processing conditions on the film structure and properties were investigated. Solutions were synthesized by mixing and reacting Zr acetylacetonate and Pb acetate trihydrate with a solution prepared from Ti isopropoxide, acetic acid and water. Chemical changes in the solution during preparation and solution storage (i.e., aging) were investigated by visual observation and FTIR, and were evidenced by changes in phase content and properties of the final PZT films. Results suggest that Zr acetylacetonate and Pb acetate trihydrate react with a Ti oxoacetate-based precursor, and that this reaction continues during aging at room temperature. The PZT film quality and properties improved with aging time of the solution before deposition. To achieve good properties and design a convenient processing route, an accelerated aging scheme, including a brief aging at 60 °C and freezing to prevent further reaction, was developed. PZT films prepared from these solutions had average dielectric constants of approximately 1040, loss tangents of approximately 0.05, remnant polarizations of approximately 26 μC/cm2, and coercive fields of approximately 39 kV/cm.